JP2011159635A - Solid lithium secondary battery and method for manufacturing the same - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide a solid lithium secondary battery where internal short-circuit and fall-off of a current collector are suppressed. <P>SOLUTION: A solid electrolyte layer and solid-state electrode layer are formed inside a frame of an electric insulation properties and the current collector is held by the frame of the electric insulation properties, thereby suppressing displacement or fall-off of the current collector. Preferably, powder, which is a material of the electrode layer is filled between the current collector and the frame to hold the current collector to the frame. <P>COPYRIGHT: (C)2011,JPO&INPIT

Description

The present invention relates to a solid-state lithium secondary battery and a method for manufacturing the same.

Lithium secondary batteries have high energy density and can output high voltages, so they are expected as power sources for batteries for electric vehicles and hybrid vehicles, and portable electric devices such as notebook computers and mobile phones. In recent years, a solid lithium secondary battery using a solid electrolyte instead of a liquid electrolyte has been proposed as a lithium secondary battery. Solid lithium secondary batteries are considered to be excellent in safety and productivity, and are expected as future secondary batteries. A solid lithium secondary battery has a structure in which a positive electrode layer, a solid electrolyte layer, and a negative electrode layer are sequentially laminated, and current collectors are attached to both sides thereof, and is generally formed by a powder forming method. That is, a positive electrode material, an electrolyte material, and a negative electrode material are placed in a mold and pressed to create a pellet in which the electrode layer and the electrolyte layer have a laminated structure (hereinafter sometimes referred to as an electrolyte electrode laminate). After the battery is taken out of the mold, a current collector plate is attached to manufacture a battery.

When manufacturing a solid lithium secondary battery as described above, since the side surface of the pellet rubs against the inner surface of the mold when taking out from the mold, the electrode material adheres to the side surface of the electrolyte layer, and the battery is internally short-circuited. There was a problem of waking up. For this reason, a solid lithium secondary battery has been proposed in which an electrode layer and an electrolyte layer are integrally formed therein using an electrically insulating frame (see Patent Document 1 below). According to this solid lithium secondary battery, since the side surface of the pellet is not rubbed, an internal short circuit of the battery can be prevented. By the way, in order to manufacture a battery, it is necessary to attach a current collecting plate to a laminate composed of a positive electrode layer, an electrolyte layer, and a negative electrode layer as described above. When the current collector plate is detached from the electrolyte electrode laminate or the adhesion area with the electrode layer is reduced, problems such as a decrease in productivity and an increase in contact resistance may occur. Therefore, it is necessary to take some means to fix the electrolyte electrode laminate and the current collector plate.

Japanese Patent Laid-Open No. 9-35724 JP 2003-168416 A JP-A-11-97072

The present invention has been made in view of the above problems, and in a solid lithium secondary battery using an electrically insulating frame, the current collector plate is detached from the electrolyte electrode laminate or the contact area with the electrode layer It is an object of the present invention to provide a solid lithium secondary battery and a method for manufacturing the same, which can suppress a decrease in battery life (hereinafter referred to as dropout).

In order to solve the above problems, the first invention is a solid lithium secondary battery,
An electrically insulating and cylindrical insulating frame;
A solid electrolyte layer formed inside the insulating frame;
An electrode layer laminated on at least one surface of the solid electrolyte layer and formed inside the insulating frame;
A current collecting member laminated on the electrode layer and held by the insulating frame;
It is characterized by providing.

According to a second invention, in the first invention,
The electrode layer is
A positive electrode layer formed by compressing powder, laminated on one of the electrolyte layers inside the insulating frame;
A negative electrode layer formed by compressing a powder layered on the other of the electrolyte layers inside the insulating frame;
Including
The current collecting member is
A positive electrode current collecting member laminated on the positive electrode layer and held by the insulating frame;
A negative electrode current collecting member laminated on the negative electrode layer and held by the insulating frame;
It is characterized by including.

According to a third invention, in the first or second invention,
The current collector plate is disposed so that at least a part thereof is within the insulating frame,
The insulating frame and an outer peripheral side surface of the current collecting member are filled with powder that is a material of an electrode layer in contact with the current collecting member.

According to a fourth invention, in the third invention,
The outer diameter of the current collecting member is smaller in the range of 200 to 1200 micrometers than the inner diameter of the insulating frame.

The fifth invention is an electrode layer material laminated on at least one surface of an electrically insulating and cylindrical insulating frame, a solid electrolyte layer formed inside the insulating frame, and at least one surface of the solid electrolyte layer. A solid lithium battery comprising: an electrode layer formed inside the insulating frame by pressing powder; and a current collecting member stacked on the electrode layer and disposed at least partially inside the insulating frame. A manufacturing method of
Pressing the material of the electrode layer by applying a force to the current collecting member, and pressing the current collecting member so as to move relative to the insulating frame during the pressing. It is characterized by including.

A sixth invention is a method of manufacturing a solid lithium secondary battery,
Put the powder, which is the material of the electrode layer, and the powder, which is the material of the electrolyte layer, into a cylindrical insulating frame that is electrically insulating, and perform temporary pressing, and from the laminated structure of the electrode layer and the electrolyte layer Forming an electrolyte electrode laminate,
Laminating the current collecting member on the electrolyte electrode laminate so that at least a part of the current collecting member is disposed in the insulating frame;
Pressing the electrolyte electrode laminate in which the current collecting member is laminated so that the current collecting member moves relative to the insulating frame;
It is characterized by including.

A seventh invention is the fifth or sixth invention, wherein
The distance that the current collecting member moves with respect to the insulating frame is not less than one fifth of the thickness of the current collector and not more than the thickness of the current collector plate.

The eighth invention is an electrode layer material laminated on at least one surface of an electrically insulating and cylindrical insulating frame, a solid electrolyte layer formed inside the insulating frame, and at least one surface of the solid electrolyte layer. A solid lithium battery comprising: an electrode layer formed inside the insulating frame by pressing powder; and a current collecting member stacked on the electrode layer and disposed at least partially inside the insulating frame. A manufacturing method of
A step of pressing the material of the electrode layer by applying a force to the current collecting member, and the electrode layer is formed by plastically deforming a layer of the powder as the material of the electrode during the pressing. Including the step of pressing the material so that the material enters between the outer periphery of the current collecting member and the insulating frame.

A ninth invention is a method of manufacturing a solid lithium secondary battery,
Put the powder, which is the material of the electrode layer, and the powder, which is the material of the electrolyte layer, into a cylindrical insulating frame that is electrically insulating, and perform temporary pressing, and from the laminated structure of the electrode layer and the electrolyte layer Forming an electrolyte electrode laminate,
Laminating the current collecting member on the electrolyte electrode laminate so that at least a part of the current collecting member is disposed in the insulating frame;
The electrode layer is plastically deformed so that the material of the electrode layer enters between the outer periphery of the current collecting member and the insulating frame, and this press is performed on the electrolyte electrode laminated body in which the current collecting members are laminated. Process,
It is characterized by including.

In a tenth aspect of the invention according to any one of the fifth to ninth aspects of the invention,
The electrode layer is
A positive electrode layer formed on one of the electrolyte layers inside the insulating frame;
A negative electrode layer formed on the other of the electrolyte layers inside the insulating frame;
Including
The current collecting member is
A positive electrode current collecting member laminated on the positive electrode layer and held by the insulating frame;
A negative electrode current collecting member laminated on the negative electrode layer and held by the insulating frame;
It is characterized by including.

In an eleventh invention according to any one of the fifth to tenth inventions,
The outer diameter of the current collecting member is smaller in the range of 200 to 1200 micrometers than the inner diameter of the insulating frame.

At least a part of the invention is an all-solid-state lithium battery comprising a solid electrolyte layer, an electrode layer, a current collecting member, and an insulating frame that covers at least the side surfaces of the solid electrolyte layer and the electrode electrode layer, It can also be said that the current collecting member is an all-solid lithium battery characterized by being held by the insulating frame. In addition, at least a part of the invention includes a solid electrolyte layer, an electrode layer formed by compressing powder, a current collector laminated on the electrode layer, at least a part of an outer periphery of the current collector, and the It can also be said that this is an all-solid-state lithium battery comprising: an electrically insulating frame covering the outer periphery of the electrolyte layer, and the frame holding the current collector. In addition, at least a part of the invention includes a solid electrolyte layer, a negative electrode layer formed by compressing powder on one side of the solid electrolyte layer, and powder on the other side of the solid electrolyte layer. A positive electrode layer formed by compression, a current collector laminated on a side of the electrode layer opposite to the side in contact with the solid electrolyte layer, at least a part of an outer circumference of the current collector and an outer circumference of the electrolyte layer It can be said that this is an all-solid-state lithium battery comprising an electrically insulating frame to be covered and the frame holding at least one of the current collectors.

According to the first or second invention, since the current collector plate is held by the insulating frame, it is possible to prevent the current collector from dropping off.

According to 3rd invention, the powder which is a material of an electrode layer is filled between the frame and the current collector. Therefore, the current collector is fixed to the insulating frame by the elastic force of the powder. Accordingly, it is possible to effectively prevent the current collector from falling off. That is, in the present invention, the current collector is indirectly held by the insulating frame via the electrode material powder.

According to the fourth aspect of the invention, the gap into which the electrode material powder enters is formed between the frame and the current collector, and the current collector is held by the elastic force of the powder filled in the gap.

According to the fifth to eighth inventions, when the press is performed, the powder as the electrode material enters between the current collector and the frame. Therefore, the solid lithium secondary battery in which the current collector is held by the frame body through the elastic force of the powder can be manufactured.

According to the ninth invention, the gap into which the powder of the electrode material enters is formed between the frame and the current collector, so that the present press can more reliably provide the electrode material between the frame and the current collector. A powder is filled.

1 is a perspective view of a solid state battery of Embodiment 1. FIG. 2 is a cross-sectional view of the solid state battery of Embodiment 1. FIG. 2 is a cross-sectional view and a partially enlarged view of the solid state battery of Embodiment 1. FIG. FIG. 3 is a diagram for illustrating the method for manufacturing the solid state battery of the first embodiment. FIG. 3 is a diagram for illustrating the method for manufacturing the solid state battery of the first embodiment. FIG. 3 is a diagram for illustrating the method for manufacturing the solid state battery of the first embodiment. FIG. 3 is a diagram for illustrating the method for manufacturing the solid state battery of the first embodiment. 6 is a perspective view of a modification of the solid state battery of Embodiment 1. FIG.

Hereinafter, embodiments of the present invention will be described with reference to the drawings.

Embodiment 1 FIG.
[Configuration of Embodiment 1]
FIG. 1 is a perspective view showing a solid lithium secondary battery according to Embodiment 1 of the present invention. As shown in FIG. 1, the solid lithium secondary battery 10 according to the present embodiment includes an electrically insulating frame 12 (hereinafter referred to as an insulating frame 12). The insulating frame 12 includes all of the side surfaces of an electrolyte layer, a positive electrode layer, and a negative electrode layer, which will be described later, a part of a side surface of the negative electrode current collector plate 14, and a side surface of the positive electrode current collector plate 16. It is provided so as to cover the part.

FIG. 2 is a cross-sectional view of the solid lithium secondary battery 10 of the present embodiment. As shown in FIG. 2, the lithium secondary battery 10 according to the present embodiment includes a laminate (electrolyte layer 20, negative electrode layer 22, and positive electrode layer 24 (hereinafter collectively referred to as an electrode layer) ( The current collector plates 14 and 16 are attached to the electrolyte electrode laminate. The insulating frame 12 is disposed so as to cover all the side portions of the electrolyte layer 20 and the electrode layers 22 and 24 and part of the side surfaces of the current collector plates 14 and 16. The electrolyte layer and the electrode layer are all made of a solid substance, and are formed by pressing a powder of the material.

In the present embodiment, the material of the electrolyte layer is 70Li2S-30P2S5, the material of the positive electrode layer is a mixture of LiCoO2 as the positive electrode active material and 70Li2S-30P2S5 as the material of the electrolyte layer, and the material of the negative electrode layer Is a mixture of graphite as the negative electrode active material and 70Li2S-30P2S5 as the material of the electrolyte layer. In the present embodiment, 70Li2S-30P2S5 uses powder having an average particle diameter of 20 micrometers, LiCoO2 uses an average particle diameter of 10 micrometers, and graphite uses an average particle diameter of 10 micrometers. The insulating frame is made of an electrically insulating resin. The current collector plate is a stainless steel plate having a thickness of 300 micrometers.

FIG. 3 is a cross-sectional view of the solid lithium secondary battery 10 of the present embodiment and an enlarged view of a part thereof. As shown in FIG. 3, the material constituting the positive electrode layer 24 (that is, the positive electrode) is formed in the gap 30 between the insulating frame 12 of the solid lithium secondary battery 10 of the present embodiment and the side surface portion of the positive electrode current collector plate 16. Active material or electrolyte layer material). Similarly, the gap between the insulating frame 12 and the negative electrode current collector plate 14 is filled with a material constituting the negative electrode layer 22 (that is, a negative electrode active material or an electrolyte layer material).

In the present embodiment, the gap 30 is set to have a width of 150 micrometers. That is, the sizes of the insulating frame 12 and the positive electrode current collector plate 16 are determined so that the difference between the inner diameter of the insulating frame 12 and the outer diameter of the positive electrode current collector plate 16 is 300 micrometers. Similarly, the size of the negative electrode current collector plate 14 is determined so that the difference between the inner diameter of the insulating frame 12 and the outer diameter of the negative electrode current collector plate 14 is 300 micrometers. As described above, the gaps 30 formed between the insulating frame 12 and the current collector plates 14 and 16 are filled with the material of the electrode layers 22 and 24, respectively. In the solid lithium secondary battery 10 of the present embodiment, the current collector plates 14 and 16 are held by the elastic force of the electrode material filled between the insulating frame 12 and the current collector plates 14 and 16 and fixed to the insulating frame. Has been. From this point of view, the insulating frame 12 holds the current collecting plates 14 and 16 via the electrode material. It can also be considered that the current collector plate is fixed to the insulating frame by the elastic force of the electrode material.

[Method for Manufacturing Solid Lithium Secondary Battery of Embodiment 1]
With reference to FIGS. 4-7, an example of the manufacturing method of the solid lithium secondary battery of this Embodiment is demonstrated. As shown in FIG. 4, first, the insulating frame 50 is set in a press device 41 for manufacturing a battery.

Next, as shown in FIG. 5, 70Li 2 S-30P 2 S 5, which is an electrolyte material, is placed in an insulating frame 50 and temporarily pressed to form an electrolyte layer 52. Furthermore, as shown in FIG. 6, a mixed material of LiCoO 2 that is a positive electrode active material and 70Li 2 S-30P 2 S 5 that is an electrolyte material is formed on one side of the electrolyte layer 52, and 70 Li 2 S-30P 2 S 5 that is an electrolyte material is formed on the other side. Each mixed material is laminated and temporarily pressed. Thus, temporary pressing is performed to form a laminate (electrolyte electrode laminate) of the positive electrode layer, the electrolyte layer, and the negative electrode layer in the insulating frame 50. At this time, the temporary press pressure is set so that the electrode layers are compressed by about 100 micrometers at the time of the main press described later.

Next, as shown in FIG. 7, current collector plates are attached to both sides of the electrolyte electrode laminate. In a state where current collector plates are attached to both sides of the electrolyte electrode laminate, pressing is performed by applying force to the current collector plates from both sides (main press). The press is applied with a force of 5 tons per square centimeter from both sides. Here, the pressing is performed such that the current collector plates 60 and 62 move relative to the insulating frame 50, respectively. That is, the current collector plates 60 and 62 are pressed so as to move inside the insulating frame 50 toward the electrolyte layer 52.

As described above, when pressing is performed so that the current collector plate moves relative to the insulating frame, the electrode layer is plastically deformed, and the material of the electrode layer is formed in the gap between the current collector plates 60 and 62 and the insulating frame 50. Enters. In other words, the material of the electrode layer is filled in the gap between the current collector plates 60 and 62 and the insulating frame 50 by displacing the current collector plate so as to dig into the electrode layer while compressing the electrode layer. . The current collecting plate is held by the elastic force of the electrode layer material. In the present embodiment, as described above, the thickness of the current collector plate is 300 micrometers, and this press was performed so that both the current collector plates 60 and 62 moved by 100 micrometers. Thus, in this embodiment, the electrode layer material is filled between the side surface of the current collector plate and the insulating frame.

[Operation and Effect of Embodiment 1]
According to the solid lithium secondary battery of the present embodiment, since the current collector plate is held by the insulating frame, the current collector plate is prevented from dropping off. If the current collector plate falls off during production, the productivity decreases, and if it falls off after production, charging / discharging becomes difficult. According to the solid lithium secondary battery of this embodiment, the current collector plate can be prevented from falling off. Therefore, these inconveniences can be suppressed. Further, if the contact pressure or contact area between the electrode layer and the current collector plate decreases without dropping, the contact resistance increases. According to the all-solid lithium secondary battery of the present invention, the current collector plate Since it can suppress moving with respect to an insulating frame, it can also suppress that the contact of an electrode layer and a current collecting plate becomes weak.

Further, according to the solid lithium secondary battery of the present embodiment, the sizes of the insulating frame and the current collecting plate are determined so that the difference between the inner diameter of the insulating frame and the outer diameter of the current collecting plate is 300 micrometers. is doing. As described above, since the average particle size of the electrode material used in this example is 10 to 20 micrometers, if there is a gap of about 150 micrometers between the insulating frame and the side surface of the current collector plate, A sufficient amount of electrode material can be filled to hold the current collector plate in the gap. Therefore, the current collector plate is held by the elastic force of the electrode material filled in the gap between the insulating frame and the current collector plate.

In addition, since the electrode material is filled in the gap between the insulating frame and the current collector plate, the electrode material in the electrode layer does not come into contact with the outside air. In general, the electrode layer is highly reactive and may be deteriorated by contact with the outside air. However, according to this embodiment, the electrode layer is not exposed to the outside air, which is preferable. Although it is conceivable to use a sealing material or the like in order to ensure hermeticity, as described above, since the electrode layer is highly reactive, a resin or the like different from the electrode material is brought into contact with the electrode layer. There is a risk of unexpected reaction. On the other hand, in this embodiment, the material of the electrode layer is used to ensure airtightness and no other type of sealing material is used, so that an unexpected reaction does not occur.

Moreover, it is also conceivable to use an adhesive as a method of fixing the insulating frame and the current collector plate. However, as described above, if a resin or the like of a material different from the electrode material is brought into contact with the electrode layer, an unexpected reaction may occur. In contrast, in the present embodiment, the current collector plate is fixed to the insulating frame without using another type of adhesive, so that the insulating frame and the current collector plate can be fixed while suppressing an unexpected reaction.

Further, as shown in FIG. 1, a part of the current collector plate is inserted into the insulating frame, and a part of the current collector plate is outside the insulating frame. Therefore, it is possible to easily attach a mechanism for extracting output from the battery, and productivity is improved. Moreover, since the electrode material is filled between the current collector plate and the insulating frame for the current collector plates on both sides, dropping off or the like is suppressed for any current collector plate.

In addition, since the pressing step and the step of filling the electrode layer material between the insulating frame and the current collector plate can be performed at the same time, manufacturing is easy. Moreover, since an insulating board can be hold | maintained in the pressed state, it can fix with applying appropriate pressure. Therefore, a solid lithium secondary battery with reduced contact resistance can be manufactured.

[Variation 1 of Embodiment 1]
In the first embodiment, the sizes of the insulating frame and the current collector plate are determined so that the difference between the inner diameter of the insulating frame and the outer diameter of the current collector plate is 300 micrometers, but the present invention is not limited to this. If the size is set so that the material of the electrode layer can enter between the insulating frame and the current collector, and the current collector can be held by the elastic force of the material of the electrode layer Good. Specifically, the gap between the side surface of the current collector plate and the insulating frame is preferably 50 micrometers to 600 micrometers, more preferably 100 micrometers to 600 micrometers. That is, it is preferable that the outer diameter of the current collector plate is smaller than the inner diameter of the insulating frame by 100 micrometers to 1200 micrometers, more preferably 200 micrometers to 1200 micrometers.

Note that the ease with which the material of the electrode layer enters the insulating frame and the current collector plate is considered to depend on the particle size of the material. Therefore, the difference between the inner diameter of the insulating frame and the outer diameter of the current collector may be determined based on the particle size of the electrode layer material. Specifically, the gap between the side surface of the current collector plate and the insulating frame is about 2 to 30 times the average particle size of the electrode layer material (the difference in diameter is 4 to 60 times the average particle size). Preferably there is. Depending on the manufacturing method of the electrode layer material, a material having a particle size larger than the average particle size may be mixed in the material. In such a case, the size of the gap may be set based on the maximum particle size of the material substance of the electrode layer. Specifically, the gap between the side surface of the current collector plate and the insulating frame is preferably about 1 to 10 times the maximum particle size (the difference in diameter is 2 to 20 times the maximum particle size). .

[Modification 2 of Embodiment 1]
In the first embodiment, the current collector plate is held by the elastic force of the material substance of the electrode layer. However, the present invention is not limited to this. It is sufficient if the current collector plate is held or fixed by an insulating frame. For example, the current collector plate may be directly held by an insulating frame. Specifically, the outer diameter of the current collector plate and the inner diameter of the insulating frame may be approximately the same. Thereby, a current collection board can be directly hold | maintained with an insulating frame, and the airtightness of an electrode layer can be ensured. That is, from the viewpoint of suppressing the falling off of the current collector plate, the current collector plate may be held by the insulating frame directly or indirectly.

[Modification 3 of Embodiment 1]
In Embodiment 1, a cylindrical insulating frame having a circular cross section is used. However, the present invention is not limited to this. That is, it is sufficient if it is made of an electrically insulating member, can form the electrolyte electrode laminate inside, and can hold the current collector plate directly or indirectly. For example, the shape may be a hollow cylinder (square cylinder) with a rectangular cross section, or a cylindrical shape with a polygonal cross section or an ellipse. That is, in the present application, the “cylindrical shape” is not limited to a circular shape.

[Modification 4 of Embodiment 1]
In the first embodiment, as shown in FIG. 1, a part of the current collector plate in the thickness direction is inside the insulating frame and a part is outside the insulating frame, but the present invention is not limited to this. For example, as shown in FIG. 8, a structure in which the current collector plate is contained in the insulating frame 72 may be adopted. In this case, it is preferable in that dropout can be suppressed even when a lateral force is applied to the battery. In the first embodiment, both current collector plates of the negative electrode and the positive electrode are held by the insulating frame. However, the present invention is not limited to this. The configuration may be applied to at least one of the current collector plates. Therefore, for example, in the case of a solid battery having a configuration in which the electrode layer of one negative electrode also serves as a negative electrode current collector, the present invention may be applied to the positive electrode side.

[Modification 5 of Embodiment 1]
In Embodiment 1, LiCoO2 is used as the positive electrode active material, 70Li2S-30P2S5 is used as the electrolyte material, graphite is used as the negative electrode active material, and stainless steel is used as the current collector plate. However, the present invention is not limited thereto. The current collector plate may be an electrically conductive substance having a strength that can be directly or indirectly held by an insulating frame. For example, aluminum, nickel, copper, or the like may be used.

The electrode active material and the electrolyte material are sufficient if they can constitute a solid lithium secondary battery. For example, TiS2 or LiNiO2 can be used as the positive electrode active material. Moreover, as a negative electrode active material, Li metal, a Li-Al alloy, a Li-In alloy etc. can be used, for example. Further, for example, Li3PO4-Li2S-SiS2 glass, Li2O, Li2SO4, Li2CO3 are used as electrolyte materials. Chalcogenite lithium ion conductors, lithium halide-containing materials, and other oxide lithium ion conductors Other solid electrolytes can be used.

Further, the particle diameters of the electrode active material and the electrolyte material are not limited to those in the first embodiment, and may be appropriately selected from the viewpoint of productivity.

[Modification 6 of Embodiment 1]
In the manufacturing method of the first embodiment, the current press is performed so that the current collector plate moves by 100 micrometers, but the present invention is not limited to this. The amount of movement may be determined so that the material of the electrode layer is filled to the extent that the current collector plate can be held by the elastic force of the material of the electrode layer. From the viewpoint of holding the current collector plate with the elastic force of the material of the electrode layer, the moving distance of the current collector plate with respect to the insulating frame is at least one fifth of the thickness of the current collector plate, Or less. That is, the temporary press pressure and the main press pressure are determined so that the moving distance of the current collector plate with respect to the insulating frame is not less than one fifth of the thickness of the current collector plate and not more than the thickness of the current collector plate. do it.

Moreover, in the manufacturing method of Embodiment 1, although temporary pressing was performed, it is not restricted to this. That is, the feature of this manufacturing method is that the material constituting the electrode layer is filled between the insulating frame and the outer periphery of the current collector plate by applying a force to the current collector plate and performing pressing. Any manufacturing method that can achieve this effect is sufficient. That is, the temporary pressing may not be performed. In addition, since the material of an electrode layer is temporarily fixed by performing a temporary press, it is preferable to perform a temporary press from a viewpoint of productivity.

DESCRIPTION OF SYMBOLS 10 Solid lithium secondary battery 12, 50, 72 Insulation frame 14, 16, 60, 62 Current collecting plate 20, 52 Electrolyte layer 22, 54 Negative electrode layer 24, 56 Positive electrode layer 30 Gap 41 Press apparatus for battery manufacture

Claims (11)

An electrically insulating and cylindrical insulating frame; a solid electrolyte layer formed inside the insulating frame; and an electrode layer formed on at least one surface of the solid electrolyte layer and formed inside the insulating frame; the laminated on the electrode layer, a solid lithium secondary battery and a current collecting member which is held by said insulating frame,
The current collector plate is at least partially fixed in the insulating frame,
The current collector plate is formed of at least one metal selected from the group consisting of stainless steel, aluminum, nickel, and copper, and is a solid lithium secondary battery . The electrode layer is laminated on one side of the electrolyte layer inside the insulating frame and is formed by compressing powder, and is laminated on the other side of the electrolyte layer inside the insulating frame. A negative electrode layer formed by compressing
The current collecting member includes: a positive electrode current collecting member laminated on the positive electrode layer and held by the insulating frame; and a negative electrode current collecting member laminated on the negative electrode layer and held by the insulating frame. 2. The solid lithium secondary battery according to 1. The current collector plate is disposed so that at least a part thereof is within the insulating frame,
3. The powder according to claim 1, wherein a powder which is a material of an electrode layer in contact with the current collecting member is filled between the insulating frame and an outer peripheral side surface of the current collecting member. Solid lithium battery. The solid lithium battery according to claim 3, wherein an outer diameter of the current collecting member is smaller than an inner diameter of the insulating frame in a range of 200 to 1200 micrometers. An electrically insulating and cylindrical insulating frame, a solid electrolyte layer formed inside the insulating frame, and a powder that is laminated on at least one surface of the solid electrolyte layer and is a material for the electrode layer is pressed. A solid lithium battery manufacturing method comprising: an electrode layer formed inside the insulating frame; and a current collecting member stacked on the electrode layer and disposed at least partially inside the insulating frame. ,
A step of pressing the material of the electrode layer by applying a force to the current collecting member, wherein the current collecting member moves inside the insulating frame toward the solid electrolyte layer during the pressing. The manufacturing method of the said solid lithium secondary battery including the said process fixed in an insulating frame by pressing. Put the powder, which is the material of the electrode layer, and the powder, which is the material of the electrolyte layer, into a cylindrical insulating frame that is electrically insulating, and perform temporary pressing, and from the laminated structure of the electrode layer and the electrolyte layer Forming an electrolyte electrode laminate,
Laminating the current collecting member on the electrolyte electrode laminate so that at least a part of the current collecting member is disposed in the insulating frame;
The current collecting member is pressed in such a manner that the current collecting member moves inside the insulating frame toward the solid electrolyte layer, thereby fixing the electrolyte electrode laminated body in which the current collecting member is laminated and the current collecting member is laminated. A process for producing a solid lithium secondary battery. The distance by which the current collecting member moves with respect to the insulating frame is not less than one fifth of the thickness of the current collecting material and not more than the thickness of the current collecting plate. The manufacturing method as described in. An electrically insulating and cylindrical insulating frame;
A solid electrolyte layer formed inside the insulating frame;
An electrode layer that is laminated on at least one surface of the solid electrolyte layer and formed inside the insulating frame by pressing powder that is a material of the electrode layer; and
A current collecting member laminated on the electrode layer, at least a part of which is disposed inside the insulating frame;
A method for producing a solid lithium battery comprising:
A step of pressing the material of the electrode layer by applying a force to the current collecting member, and the electrode layer is formed by plastically deforming a layer of the powder as the material of the electrode during the pressing. A method for producing a solid lithium secondary battery including the above step, wherein the material is pressed so as to enter between the outer periphery of the current collecting member and the insulating frame. Put the powder, which is the material of the electrode layer, and the powder, which is the material of the electrolyte layer, into a cylindrical insulating frame that is electrically insulating, and perform temporary pressing, and from the laminated structure of the electrode layer and the electrolyte layer Forming an electrolyte electrode laminate,
Laminating the current collecting member on the electrolyte electrode laminate so that at least a part of the current collecting member is disposed in the insulating frame;
The electrode layer is plastically deformed so that the material of the electrode layer enters between the outer periphery of the current collecting member and the insulating frame, and this press is performed on the electrolyte electrode laminated body in which the current collecting members are laminated. Process,
Of manufacturing a solid lithium secondary battery. The electrode layer includes a positive electrode layer formed on one of the electrolyte layers inside the insulating frame, and a negative electrode layer formed on the other of the electrolyte layers inside the insulating frame,
The current collecting member includes a positive electrode current collecting member laminated on the positive electrode layer and held by the insulating frame, and a negative electrode current collecting member laminated on the negative electrode layer and held by the insulating frame. Item 10. The method for producing a solid lithium secondary battery according to any one of Items 5 to 9. The manufacturing method according to claim 5, wherein an outer diameter of the current collecting member is smaller than an inner diameter of the insulating frame in a range of 200 to 1200 micrometers.

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